Wang Zhongke, Zhang Qixing, Gao Jing, Wang Jin, He Han, Pan Sanjiang, Zhao Ying, Zhang Xiaodan
Institute of Photoelectronic Thin Film Devices and Technology, Renewable Energy Conversion and Storage Center, State Key Laboratory of Photovoltaic Materials and Cells, Nankai University, Tianjin, 300350, P. R. China.
Tianjin Key Laboratory of Efficient Utilization of Solar Energy, Tianjin, 300350, P. R. China.
Small. 2025 Jul;21(30):e2502144. doi: 10.1002/smll.202502144. Epub 2025 May 27.
During coupling with carbon dioxide reduction reactions (CO₂RR), plastic reforming as an effective alternative anodic reaction to replace oxygen evolution reaction (OER), offers dual benefits of reducing energy consumption and producing valuable chemicals. However, balancing the energy requirements of polyethylene terephthalate (PET) oxidation with CO₂RR is challenging, as both half-reactions must operate under compatible conditions for high efficiency. Here, it is developed a bifunctional copper hydroxide catalyst capable of simultaneously converting both PET and CO₂ into valuable chemicals, which simplifies the system complexity. The copper hydroxide-derived catalyst achieves a formate FE of 89.5% produced on anode and an ethylene FE of 60.8% on cathode. It is discovered that CuOOH forms when Cu(OH)₂ is immersed in an EG electrolyte, enhancing EG adsorption and promoting its oxidation. After pre-reduction, the Cu(OH)₂-derived catalyst shows increased exposure of Cu(100) facets and enhanced C-C coupling for CO₂ reduction to ethylene. Driven by a silicon solar cell module, the product formation rates of 4.72 mmol/h/cm (formate) and 9.65 mmol/h/cm (ethylene) is achieved by the system at a current density of 302.7 mA/cm. This work proposes a sustainable strategy utilizing a bifunctional catalyst for solar electrochemical upcycling of PET plastic, coupled with CO₂ reduction, to generate value-added fuels.
在与二氧化碳还原反应（CO₂RR）耦合过程中，塑料重整作为一种有效的替代阳极反应来取代析氧反应（OER），具有降低能耗和生产有价值化学品的双重好处。然而，平衡聚对苯二甲酸乙二酯（PET）氧化与CO₂RR的能量需求具有挑战性，因为两个半反应都必须在兼容条件下高效运行。在此，开发了一种双功能氢氧化铜催化剂，能够同时将PET和CO₂转化为有价值的化学品，从而简化了系统复杂性。由氢氧化铜衍生的催化剂在阳极上产生的甲酸盐法拉第效率（FE）为89.5%，在阴极上产生的乙烯FE为60.8%。研究发现，当Cu(OH)₂浸入乙二醇（EG）电解液中时会形成CuOOH，增强了EG的吸附并促进其氧化。预还原后，由Cu(OH)₂衍生的催化剂显示出Cu(100)晶面的暴露增加，以及用于将CO₂还原为乙烯的C-C偶联增强。在硅太阳能电池模块的驱动下，该系统在电流密度为302.7 mA/cm²时实现了4.72 mmol/h/cm²（甲酸盐）和9.65 mmol/h/cm²（乙烯）的产物生成速率。这项工作提出了一种可持续策略，利用双功能催化剂对PET塑料进行太阳能电化学升级循环，同时结合CO₂还原，以生成增值燃料。
